EP0977294A1 - Installation de piles à combustible fonctionnant à haute température - Google Patents

Installation de piles à combustible fonctionnant à haute température Download PDF

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Publication number
EP0977294A1
EP0977294A1 EP99810576A EP99810576A EP0977294A1 EP 0977294 A1 EP0977294 A1 EP 0977294A1 EP 99810576 A EP99810576 A EP 99810576A EP 99810576 A EP99810576 A EP 99810576A EP 0977294 A1 EP0977294 A1 EP 0977294A1
Authority
EP
European Patent Office
Prior art keywords
reformer
fuel
fuel cells
reforming
gas
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
EP99810576A
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German (de)
English (en)
Other versions
EP0977294B1 (fr
Inventor
Alexander Dr. Schuler
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Hexis AG
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Hexis AG
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Filing date
Publication date
Application filed by Hexis AG filed Critical Hexis AG
Priority to EP99810576A priority Critical patent/EP0977294B1/fr
Publication of EP0977294A1 publication Critical patent/EP0977294A1/fr
Application granted granted Critical
Publication of EP0977294B1 publication Critical patent/EP0977294B1/fr
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
    • H01M8/0625—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material in a modular combined reactor/fuel cell structure
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2465—Details of groupings of fuel cells
    • H01M8/247—Arrangements for tightening a stack, for accommodation of a stack in a tank or for assembling different tanks
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M2008/1293—Fuel cells with solid oxide electrolytes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H01M2300/0071—Oxides
    • H01M2300/0074—Ion conductive at high temperature
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04007—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids related to heat exchange
    • H01M8/04014—Heat exchange using gaseous fluids; Heat exchange by combustion of reactants
    • H01M8/04022—Heating by combustion
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the invention relates to a system with high-temperature fuel cells according to the preamble of claim 1 and a method for operating the Investment.
  • This device contains a cell block Fuel cells that are surrounded by a heat-insulating shell.
  • the post-combustion chamber is located between the casing and the cell block.
  • Fuel gas reformer also called prereformer
  • Exhaust gases can be supplied.
  • a liquid fuel can also be provided, although the use of a liquid fuel can be associated with additional problems in that it has to be fed into the reformer in a suitable manner.
  • the object of the invention is a plant with high-temperature fuel cells to create the one for the reforming of the fuel required process heat in a beneficial for the overall process Won and fed to the reform. This task will solved by the system defined in claim 1.
  • the system contains high-temperature fuel cells that are arranged in a planar configuration in a centrally symmetrical stack.
  • a feed point is provided for a gaseous or liquid fuel.
  • the fuel can be catalytically converted at least partially into CO and H 2 in the presence of H 2 O and with the addition of process heat.
  • a central cavity is arranged along the stack axis, via which the fuel processed in the reformer can be fed into the fuel cells.
  • the reformer is arranged in the central cavity and is designed in such a way that the heat required for the endothermic reforming processes can be at least partially transferred from the fuel cells to the reformer via radiation.
  • the reformer of the system according to the invention is referred to below as integrated reformer.
  • the dependent claims 2 to 9 relate to advantageous Embodiments of the system according to the invention.
  • Subject of Claim 10 is a method for operating this system.
  • the system 1 in FIG. 1 comprises the following components: a stack 2 with planar, annular fuel cells 20 and poles 27, 28 to deliver a electrical energy E; a shell 3, the inner, not shown Structure, by means of which ambient air 80, 81 during operation is preheated and evenly distributed to the cell stack 2; on Post-combustion chamber 6 between cell stack 2 and shell 3, from the exhaust gas 60, 70 via a heat exchanger 7 (delivery of heat Q to Heat transfer medium 79 of a water cycle) is removed; a mixing organ 67, in which hot exhaust gas 60 'is combined with cooled exhaust gas 70' a return line 61 for the exhaust gas and a fan 62; further a Plant part 5, in the fuel 50 (supply line 51) with the recirculated Exhaust gas of line 61 is mixed. Following this feed point 5 the mixture is processed by reforming and the processed one Fuel 57 fed into the cells 20, which it flows through as gas 58.
  • Reforming is an endothermic process.
  • Integrated reformer 4 - see Fig. 2 - in a central cavity 25 of the Cell stack 2 arranged along the stack axis and designed so that radiated heat emitted by the cells 20 are absorbed by it can.
  • the high-temperature fuel cell 20 comprises an electrochemically active plate 21 (with two electrode layers and one solid electrolyte layer in between) and an interconnector 22, of the electrochemically active plates 21 of adjacent cells 20 connects in a leading way.
  • the interconnector 22 is used as a heat exchanger for the Heating of air 82 fed through feed lines 81 ′ is formed.
  • the heated air 83 flows radially outward parallel to the gas 58. Components of the gas 58 that have not reacted in the cell 20 are after combining with airflow 83 in post-combustion chamber 6 burned.
  • the annular space 6 is of an air-permeable wall 31, which is sealed on the inside with a layer 36.
  • Air 80 is applied to the wall 31 via a second annular space 38 distributed, pre-warmed in this and through the lines 81 'in the Interconnectors 22 fed.
  • the envelope that wall 31 and Distribution space 38 includes, is evacuated to the outside by an closed annular chamber 39.
  • Exhaust gas 60 ′, 70 ′ returned to the reformer 4 contains H 2 O, CO 2 , O 2 and N 2 .
  • the reforming of the fuel 50, the hydrocarbons z. B. C n H 2 + 2n , with n 1, 2, ..., includes endothermic reactions such as CH 4 + H 2 O ⁇ CO + 3 H 2 , C n H 2n + 2 + n H 2 O ⁇ n CO + (2n + 1) H 2 , CH 4 + CO 2 ⁇ 2 CO + 2 H 2 . Parallel to these reactions, partial oxidations, i.e.
  • FIG. 3 shows a system 1 in which part of the recirculated exhaust gas 70 'is mixed with the ambient air 80.
  • the ambient air 80 conveyed by a blower 8 serves the current-supplying processes as an O 2 -releasing and waste heat-absorbing medium.
  • the amount delivered delivers an excess of O 2 (based on the stoichiometric amount required for the processes).
  • Fig. 4 shows a feed point 5 for a liquid fuel 50, which with a Pump 52 is fed.
  • a nozzle device 54 the fuel 50 sprayed and with the recirculated exhaust gas 70 '(or 70' and 60 ') mixed.
  • the mixture produced, a spray mist 56 ′ is fed into the reformer 4 distributed, which is in the central cavity 25 of the cell stack 2 (see Figures 1 and 2).
  • the spray 56 ' is in one gas-permeable, catalyst-bearing structure 40 processed (by Reforming and / or partial oxidation).
  • This structure 40 which as 5 is shown in a concentric arrangement inner zone 40a and an outer zone 40b.
  • the outer zone is 40b evenly formed and produces a much larger radial Flow resistance than the inner.
  • the inner zone 40a is as Droplet separator designed. There the liquid phase of the Fuel 50 by evaporation or due to chemical Reactions in gaseous form. The processing is carried out in the outer zone 40b continued; at the same time, through denser zone 40b uniform distribution of the spread gas 57 'to the individual Fuel cells 20.
  • a catalyst for reforming and / or partial oxidation for example the following substances in question: platinum, palladium, ruthenium, Rhodium and nickel or a mixture of two or more of these substances.
  • nickel is less for partial oxidation due to soot formation suitable.
  • an additional water inlet (reference number 90 in FIG. 3) may be required to reduce the risk of carbon capture, i.e. Soot formation, to be able to switch off.
  • Additional water intake can be practical any ratio of reforming and partial reactions Oxidation can be adjusted to each other. Because this ratio depends If the fuel is different, the process can be optimally adapted to the respective Fuel can be adjusted. For fuels that are used only little Soot formation (natural gas, biogas, methanol) can lead to an additional Water supply can be dispensed with.
  • the integrated reformer 4 of FIGS. 2 and 4 extends essentially over the entire height of the cell stack 2.
  • a gas-permeable Structure 40 encloses a tubular distribution channel.
  • This structure 40 has an inner surface that contains a catalyst, e.g. H. catalytic, the Reforming activating substances.
  • the reformer 4 is designed such that the flow resistance along the distribution channel is significantly lower is as radial through the gas permeable structure 40 and that the radial Flow resistance essentially over the entire length of the reformer is the same size.
  • the processed, gaseous Fuel 57 evenly distributed over all cells 20.
  • the gas permeable structure 40 which forms a porous tube, is made of made of metallic and / or ceramic material.
  • This pipe points For example, an open-pore foam structure, as shown in Fig. 5 for the inner zone 40a is provided.
  • the integrated reformer 4 can, for example, also be a bundle of vertical pipes, as shown in FIGS. 6 and 7 is shown.
  • Fig. 6 shows a side view of the tube bundle
  • Fig. 7 one Cross-section.
  • the lateral boundary of the central cavity 25 is through dash-dotted lines 25 'indicated.
  • the gaseous fuel 50 fed in is preheated. After that it will preheated gas via a container 42 to a plurality of tubes 43 distributed.
  • the catalytic processes of the Implementation instead.
  • a sufficiently large one for these processes Surface is available, the tubes 43 can have a "fractal" inner surface 43i can be equipped, as indicated in Fig. 8. This surface 43i can be provided with a washcoat which carries the catalysts be coated.
  • the tubes 43 open at their upper ends in the central cavity 25, via which the gas 57 processed in the reformer 4 into the fuel cells 20 is distributed.
  • the volume of the central cavity 25 is said to be substantial be greater than the total volume of the tubes 41, 43, so that there is a largely uniform distribution of the processed gas 57 on the Fuel cells 20 results.
  • the integrated reformer 4 can be made from Stack elements 44 may be joined together, these stack elements are in particular baskets which are granules formed as catalyst supports 49 included.
  • a basket 44 includes a bottom 440 with a central one Breakthrough 441. The granulate 49 is inside and outside by vertical Pillars 441 and 442 held. It gets into basket 44 up to level 49 ' poured in.
  • the reformer 4 only needs to be designed for part of the reforming be when the gas-side electrodes of the fuel cells with catalytic effective substances, by means of which the reforming is feasible.
  • Type of Material for the catalyst support There are a large number of freely selectable parameters: Type of Material for the catalyst support, type of catalytically active coating, Porosity of the carrier, geometry (outer and inner diameter of the porous tube, ratio to the diameter of the central cavity). This enables a wide range of applications for different fuels and operational characteristics. By choosing the geometry, the transferable amount of heat can be set in a very wide range.
  • the exemplary embodiments described relate to systems in which exhaust gas is returned to the reformer. However, the invention also relates to Systems in which no exhaust gas recirculation is provided (as is the case with the aforementioned EP-A 0 780 917 is the case).
EP99810576A 1998-07-31 1999-07-02 Installation de piles à combustible fonctionnant à haute température Expired - Lifetime EP0977294B1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP99810576A EP0977294B1 (fr) 1998-07-31 1999-07-02 Installation de piles à combustible fonctionnant à haute température

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
EP98810739 1998-07-31
EP98810739 1998-07-31
EP99810576A EP0977294B1 (fr) 1998-07-31 1999-07-02 Installation de piles à combustible fonctionnant à haute température

Publications (2)

Publication Number Publication Date
EP0977294A1 true EP0977294A1 (fr) 2000-02-02
EP0977294B1 EP0977294B1 (fr) 2003-11-12

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EP99810576A Expired - Lifetime EP0977294B1 (fr) 1998-07-31 1999-07-02 Installation de piles à combustible fonctionnant à haute température

Country Status (9)

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US (1) US6274260B1 (fr)
EP (1) EP0977294B1 (fr)
JP (1) JP2000058096A (fr)
KR (1) KR20000011646A (fr)
CN (1) CN1147017C (fr)
AT (1) ATE254340T1 (fr)
AU (1) AU751579B2 (fr)
DE (1) DE59907690D1 (fr)
DK (1) DK0977294T3 (fr)

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE10013477A1 (de) * 2000-03-18 2001-10-18 Volkswagen Ag Brennstoffzellenvorrichtung und Verfahren zu dessen Betriebsdynamikverbesserung
WO2002041425A2 (fr) * 2000-11-15 2002-05-23 Mtu Friedrichshafen Gmbh Ensemble de piles a combustibles
WO2003067698A1 (fr) 2002-02-05 2003-08-14 Tokyo Gas Company Limited Systeme de pile a combustible a oxyde solide
WO2005069776A2 (fr) 2004-01-22 2005-08-04 Ion America Corporation Systeme de piles a combustible a haute temperature et procede de fonctionnement
EP1739777A2 (fr) 2005-06-28 2007-01-03 J. Eberspächer GmbH Co. KG Système de pile à combustible pour véhicules
US9941525B2 (en) 2011-01-06 2018-04-10 Bloom Energy Corporation SOFC hot box components
US9947955B2 (en) 2006-01-23 2018-04-17 Bloom Energy Corporation Modular fuel cell system

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US6090312A (en) * 1996-01-31 2000-07-18 Ziaka; Zoe D. Reactor-membrane permeator process for hydrocarbon reforming and water gas-shift reactions
US6440594B1 (en) * 1999-06-17 2002-08-27 California Institute Of Technology Aerosol feed direct methanol fuel cell
JP2003178783A (ja) * 2001-10-02 2003-06-27 Ngk Insulators Ltd 燃料電池発電装置
US20060204796A1 (en) * 2005-03-08 2006-09-14 General Electric Company Systems and Methods for Minimizing Temperature Differences and Gradients in Solid Oxide Fuel Cells
US7524572B2 (en) 2005-04-07 2009-04-28 Bloom Energy Corporation Fuel cell system with thermally integrated combustor and corrugated foil reformer
US7659022B2 (en) 2006-08-14 2010-02-09 Modine Manufacturing Company Integrated solid oxide fuel cell and fuel processor
US20090214905A1 (en) * 2007-01-08 2009-08-27 California Institute Of Technology Direct methanol fuel cell operable with neat methanol
US8920997B2 (en) 2007-07-26 2014-12-30 Bloom Energy Corporation Hybrid fuel heat exchanger—pre-reformer in SOFC systems
US8852820B2 (en) 2007-08-15 2014-10-07 Bloom Energy Corporation Fuel cell stack module shell with integrated heat exchanger
WO2009105191A2 (fr) 2008-02-19 2009-08-27 Bloom Energy Corporation Système de piles à combustible contenant un dispositif d'oxydation de gaz résiduaire d'anode et un échangeur de chaleur/reformeur hybride
JP2009245627A (ja) * 2008-03-28 2009-10-22 Mitsubishi Materials Corp 固体酸化物形燃料電池
US8968958B2 (en) 2008-07-08 2015-03-03 Bloom Energy Corporation Voltage lead jumper connected fuel cell columns
EP2534095A2 (fr) * 2010-02-13 2012-12-19 McAlister Technologies, LLC Cuves de réacteurs avec surfaces transmissives pour la production de combustibles à base d'hydrogène, éléments structuraux, systèmes et procédés associés
US8440362B2 (en) 2010-09-24 2013-05-14 Bloom Energy Corporation Fuel cell mechanical components
US9755263B2 (en) 2013-03-15 2017-09-05 Bloom Energy Corporation Fuel cell mechanical components
WO2015061274A1 (fr) 2013-10-23 2015-04-30 Bloom Energy Corporation Pré-reformeur pour le reformage sélectif d'hydrocarbures supérieurs
CN105431375B (zh) * 2013-11-01 2018-01-23 Lg化学株式会社 燃料电池及其制备方法
WO2015123304A1 (fr) 2014-02-12 2015-08-20 Bloom Energy Corporation Structure et procédé pour système de piles à combustible où plusieurs piles à combustible et une électronique de puissance alimentent des charges en parallèle permettant la spectroscopie d'impédance électrochimique (« sie ») intégrée
US10651496B2 (en) 2015-03-06 2020-05-12 Bloom Energy Corporation Modular pad for a fuel cell system
WO2019018446A1 (fr) 2017-07-17 2019-01-24 Fractal Heatsink Technologies, LLC Système et procédé pour dissipateur thermique multi-fractal
US11398634B2 (en) 2018-03-27 2022-07-26 Bloom Energy Corporation Solid oxide fuel cell system and method of operating the same using peak shaving gas

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JPS6298567A (ja) * 1985-10-25 1987-05-08 Hitachi Ltd 燃料電池
EP0398111A1 (fr) * 1989-05-18 1990-11-22 Asea Brown Boveri Ag Dispositif pour convertir de l'énergie chimique d'hydrocarbures en énergie électrique au moyen d'un procédé électrochimique à haute température
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EP0551054A1 (fr) * 1992-01-09 1993-07-14 Sulzer Innotec Ag Pile à combustible à symétrie axiale
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EP0673074A1 (fr) * 1994-02-19 1995-09-20 ROLLS-ROYCE plc Une batterie de pile à combustible à base d'oxydes solides
EP0780917A1 (fr) * 1995-12-19 1997-06-25 Sulzer Innotec Ag Dispositif comportant des piles à combustible

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EP0398111A1 (fr) * 1989-05-18 1990-11-22 Asea Brown Boveri Ag Dispositif pour convertir de l'énergie chimique d'hydrocarbures en énergie électrique au moyen d'un procédé électrochimique à haute température
EP0443241A1 (fr) * 1989-12-28 1991-08-28 Westinghouse Electric Corporation Dispositif de cellules électrochimiques comportant des entrées distribuées selon l'axe permettant l'élimination du mélange combustible-combustible usé transversalement aux longueurs des cellules
EP0551054A1 (fr) * 1992-01-09 1993-07-14 Sulzer Innotec Ag Pile à combustible à symétrie axiale
EP0635896A1 (fr) * 1993-07-20 1995-01-25 Sulzer Innotec Ag Pile à combustible à symétrie axiale
WO1995010126A1 (fr) * 1993-10-06 1995-04-13 Ceramatec, Inc. Conception modulaire d'empilements de piles a combustible d'oxyde solide cpn/reformateur integre
EP0673074A1 (fr) * 1994-02-19 1995-09-20 ROLLS-ROYCE plc Une batterie de pile à combustible à base d'oxydes solides
EP0780917A1 (fr) * 1995-12-19 1997-06-25 Sulzer Innotec Ag Dispositif comportant des piles à combustible

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Cited By (12)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE10013477A1 (de) * 2000-03-18 2001-10-18 Volkswagen Ag Brennstoffzellenvorrichtung und Verfahren zu dessen Betriebsdynamikverbesserung
WO2002041425A2 (fr) * 2000-11-15 2002-05-23 Mtu Friedrichshafen Gmbh Ensemble de piles a combustibles
WO2002041425A3 (fr) * 2000-11-15 2002-12-12 Mtu Friedrichshafen Gmbh Ensemble de piles a combustibles
WO2003067698A1 (fr) 2002-02-05 2003-08-14 Tokyo Gas Company Limited Systeme de pile a combustible a oxyde solide
EP2244327A1 (fr) * 2002-02-05 2010-10-27 Tokyo Gas Co., Ltd. Système de pile à combustible à oxyde solide
WO2005069776A2 (fr) 2004-01-22 2005-08-04 Ion America Corporation Systeme de piles a combustible a haute temperature et procede de fonctionnement
EP1754270A2 (fr) * 2004-01-22 2007-02-21 Ion America Corporation Systeme de piles a combustible a haute temperature et procede de fonctionnement
EP1754270A4 (fr) * 2004-01-22 2008-06-04 Ion America Corp Systeme de piles a combustible a haute temperature et procede de fonctionnement
EP1739777A2 (fr) 2005-06-28 2007-01-03 J. Eberspächer GmbH Co. KG Système de pile à combustible pour véhicules
EP1739777A3 (fr) * 2005-06-28 2009-01-21 J. Eberspächer GmbH Co. KG Système de pile à combustible pour véhicules
US9947955B2 (en) 2006-01-23 2018-04-17 Bloom Energy Corporation Modular fuel cell system
US9941525B2 (en) 2011-01-06 2018-04-10 Bloom Energy Corporation SOFC hot box components

Also Published As

Publication number Publication date
CN1244049A (zh) 2000-02-09
ATE254340T1 (de) 2003-11-15
CN1147017C (zh) 2004-04-21
EP0977294B1 (fr) 2003-11-12
DK0977294T3 (da) 2004-01-05
DE59907690D1 (de) 2003-12-18
JP2000058096A (ja) 2000-02-25
US6274260B1 (en) 2001-08-14
KR20000011646A (ko) 2000-02-25
AU751579B2 (en) 2002-08-22
AU4239399A (en) 2000-02-24

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